Molecularly Engineered, Multifunctional Imide Derivatives for Practical Zn Metal Full Cells
Abstract
Aqueous zinc metal batteries (ZMBs) are attractive owing to their intrinsic safety and low cost. However, the practical applications are limited by dendrite growth, hydrogen evolution reaction (HER), and corrosion. Additionally, the N/P ratio is too high to achieve a large energy density and the current rate is often restricted to ≤ 4 mA cm-2. Herein, we demonstrate multifunctional additives of imide derivatives for practical aqueous Zn metal full cells. Systematically comparing four imide derivatives to assess the role of relevant functional groups in the reversibility of Zn deposition, succinimide (H-SU) was chosen as a proof-of-concept for the molecularly engineered imide derivative additive. The H-SU additives reconstruct the solvation sheath of Zn2+ with imino groups disrupting the hydrogen bond (HB) network of free water with carbonyl groups, while they are adsorbed onto the Zn surface to adjust the inner Helmholtz plane. These combined modifications of solvated and interfacial structures by multifunctional H-SU additives led to alleviating HER and guiding uniform Zn deposition. Consequently, the H-SU additives enabled Zn||Zn symmetric cells to exhibit a long term stability over 2700 h at 1 mA cm-2 and 1 mAh cm-2, and even to achieve a record of 21000 cycles (or 700 h) at an extremely high current density of 60 mA cm-2. Furthermore, the H-SU additives optimized the battery performance of full cells integrating Zn anodes with three types of cathodes, including polyaniline (PANI), manganese vanadate, and molybdenum oxide@titanium dioxide. Particularly, the Zn||PANI full cells with a low N/P ratio of 2.2 and an ultrahigh loading of 60 mg cm-2 delivered a high areal capacity of 4.2 mAh cm-2 after 100 cycles. Therefore, this work provides insights into the molecular engineering design of multifunctional imide derivative additives and offers technical breakthrough for practical Zn metal full cells.